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Solid-state lithium metal batteries (LMBs) have become increasingly important in recent years due to their potential to offer higher energy density and enhanced safety compared to conventional liquid electrolyte-based lithium-ion batteries (LIBs). However, they require highly functional solid-state electrolytes (SSEs) and, therefore, many inorganic materials such as oxides of perovskite La_2/3−xLi_3xTiO₃ (LLTO) and garnets La₃Li₇Zr₂O₁₂ (LLZO), sulfides Li₁₀GeP₂S₁₂ (LGPS), and phosphates Li_1+xAl_xTi_2−x(PO₄)_3x (LATP) are under investigation. Among these oxide materials, LLTO exhibits superior safety, wider electrochemical window (8 V vs. Li/Li⁺), and higher bulk conductivity values reaching in excess of 10⁻³ S cm⁻¹ at ambient temperature, which is close to organic liquid-state electrolytes presently used in LIBs. However, recent studies focus primarily on composite or hybrid electrolytes that mix LLTO with organic polymeric materials. There are scarce studies of pure (100%) LLTO electrolytes in solid-state LMBs and there is a need to shed more light on this type of electrolyte and its potential for LMBs. Therefore, in our review, we first elaborated on the structure/property relationship between compositions of perovskites and their ionic conductivities. We then summarized current issues and some successful attempts for the fabrication of pure LLTO electrolytes. Their electrochemical and battery performances were also presented. We focused on tape casting as an effective method to prepare pure LLTO thin films that are compatible and can be easily integrated into existing roll-to-roll battery manufacturing processes. This review intends to shed some light on the design and manufacturing of LLTO for all-ceramic electrolytes towards safer and higher power density solid-state LMBs. Full article